量子产额
发光
光致发光
材料科学
硫族元素
热稳定性
密度泛函理论
闪烁体
产量(工程)
表面改性
纳米技术
光电子学
物理化学
结晶学
化学
计算化学
荧光
有机化学
光学
物理
冶金
探测器
作者
Rattapon Khamlue,Tomoaki Sakurada,Yeongsu Cho,Woo Seok Lee,Pimpan Leangtanom,Michael G. Taylor,Worakit Naewthong,Pongsakun Sripetch,Busayakorn Na Ranong,Tossawat Autila,Thiti Rungseesumran,J. Kaewkhao,Taweesak Sudyoadsuk,Atcha Kopwitthaya,Péter Müller,Vinich Promarak,Heather J. Kulik,William A. Tisdale,Watcharaphol Paritmongkol
标识
DOI:10.1021/acs.chemmater.4c00653
摘要
Metal organochalcogenides (MOCs) are an emerging class of luminescent hybrid organic–inorganic semiconductors, whose structures and properties can be tuned by organic functionalization and substitutions of their metal and chalcogen elements. Herein, we present a new design strategy by heterocyclic modification, resulting in the transformation of prototypical two-dimensional (2D) silver phenylselenide (AgSePh) to a zero-dimensional (0D) silver pyridinylselenide (AgSePy) via the formation of Ag–N bonds. At room temperature, AgSePy shows strong and broad orange photoluminescence (PL; λmax = 636 nm, full-width-at-half-maximum = 111 nm, quantum yield = 64%) with a large 259 nm Stoke's shift and a 3.4 μs lifetime. Using steady-state and time-resolved PL spectroscopy under varying temperature and oxygen conditions, we found AgSePy to exhibit air-stable luminescence and maintain a high PL quantum yield and a single exponential PL lifetime down to 4 K. Furthermore, AgSePy shows excellent thermal stability up to ∼250 °C and chemical stability against polar, nonpolar, and aqueous solvents at pH 3–14. Density functional theory calculations further confirm the 0D electronic structure. Finally, we successfully demonstrated the performance of AgSePy as an X-ray scintillator with an estimated light yield of ∼8,000 phe/MeV and a spatial resolution down to 0.080 ± 0.005 mm. Overall, this work provides a novel tactic to modify the structures and properties of MOCs, highlighting their structural richness and structure–property relationship, and introduces their new use as X-ray scintillators, encouraging further development in radiation detection and medical imaging.
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